Efficient NO2 gas sensors are critical for environmental monitoring and industrial safety. However, the design of reliable NO2 sensing materials with high activity and moisture resistance remains a challenge, primarily due to limited active sites and interference from high air humidity. In this paper, SnO2/ZIF-8 nanocomposites were prepared by leveraging the inherent moisture resistance and abundant active sites of ZIF-8 nanoparticles, as well as the good electronic migration capabilities of SnO2 nanospheres. The synergistic effect between metal-organic frameworks and metal oxides enables the gas sensor to show an impressive response (Rg/Ra = 85.95) to 1 ppm of NO2 even in high-humidity conditions, with good selectivity. Additionally, the SnO2/ZIF-8 composite-based chemiresistive sensors exhibit a low limitation of detection (11 ppb), fast response/recovery time (57/75 s), and excellent long-term stability (over 35 days), rendering them highly suitable for practical NO2 detection. Density functional theory (DFT) calculations have demonstrated that the loading of ZIF-8 nanoparticles can enhance the adsorption effect as well as promote charge transfer between NO2 molecules and the SnO2 nanospheres. The synthesis of this composite material provides new ideas for improving the detection ability of NO2 at high humidity.